[NEt4](2)[Tc(CO)(3)Cl-3] reacts with thiosemicarbazones derived fro 2,2'-dipyridyl ketone (HL3) and 4-acetylpyridine (HL4) to for stable technetium(l) complexes of the compositions [Tc(CO)(3)Cl-(HL3-N-py,N-py)] and [Tc-2(CO)(6)Cl-2(mu-HL4-N-py, S)]. Whereas exclusively the pyridine nitrogen atoms are involved in coordination in the monomeric complex, the binuclear compound represents the first technetium complex with a coordinated thiosemicarbazone functionality.